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Dynamical heterogeneity in binary mixtures of low-molecular-weight glass formers

Daniele Cangialosi1, Angel Alegría2, and Juan Colmenero1,2,3

  • 1Centrol de Fisica de Materiales CFM (CSIC–UPV/EHU), Apartado 1072, 20080 San Sebastián, Spain
  • 2Departamento de Física de Materiales, Universidad del País Vasco (UPV/EHU), Apartado 1072, 20080 San Sebastián, Spain
  • 3Donostia International Physics Center, Paseo Manuel de Lardizabal 4, 20018 San Sebastián, Spain

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Phys. Rev. E 80, 041505 – Published 27 October, 2009

DOI: https://doi.org/10.1103/PhysRevE.80.041505

Abstract

Homogeneous diethyl phthalate/phenylphthalein-dimethylether (DEP/PDE) mixtures have been investigated by means of broadband dielectric spectroscopy. Contrarily to the widespread view that homogenous binary mixtures should give rise to a single glass transition, the mixture displays two dynamics giving rise to two glass transitions. Such a finding can be rationalized invoking the self-concentration concept that relies on the localized nature of the glass transition phenomenon. In such a way, the analogy with miscible polymer blends, for which this concept has been introduced, is highlighted. A model based on the combination of the Adam-Gibbs (AG) theory of the glass transition and the self-concentration concept resulted to be fully predictive once the only unknown variable, namely, the glass-former specific parameter (α) connecting the characteristic length for the glass transition to the configurational entropy, is extracted applying the model itself to DEP/toluene and DEP/PDE solutions highly concentrated, respectively, in DEP and PDE. The α parameter obtained in such a way allows the precise determination of the most probable relaxation time even for those DEP/PDE mixtures displaying a strong overlap of the dielectric response. The model incorporating the self-concentration concept to the AG theory also provides the characteristic length scale for the glass transition for both DEP and PDE. Such a length scale was found to be on the order of 1–2 nm. This is comparable to that obtained for other glass formers.

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Outline

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Phys. Rev. E 80, 041505– Published 27 October, 2009
  • Received 8 June 2009

© 2009 American Physical Society

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